A better understanding of stormwater generation and solute sources is needed to improve the protection of aquatic ecosystems, infrastructure, and human health from large runoff events. Much of our understanding of water and solutes produced during stormflow comes from studies of individual, small headwater catchments. This study compared many different types of catchments during a single large event to help isolate landscape controls on streamwater and solute generation, including human-impacted land cover. We used a distributed network of specific electrical conductivity sensors to trace storm response during the post-tropical cyclone Sandy event of October 2012 at 29 catchments across the state of New Hampshire. A citizen science sensor network, Lotic Volunteer for Temperature, Electrical Conductivity, and Stage, provided a unique opportunity to investigate high-temporal resolution stream behavior at a broad spatial scale. Three storm response metrics were analyzed in this study: (a) fraction of new water contributing to the hydrograph; (b) presence of first flush (mobilization of solutes during the beginning of the rain event); and (c) magnitude of first flush. We compared new water and first flush to 64 predictor attributes related to land cover, soil, topography, and precipitation. The new water fraction was positively correlated with low and medium intensity development in the catchment and riparian buffers and with the precipitation from a rain event 9 days prior to Sandy. The presence of first flush was most closely related (positively) to soil organic matter. Magnitude of first flush was not strongly related to any of the catchment variables. Our results highlight the potentially important role of human landscape modification in runoff generation at multiple spatial scales and the lack of a clear role in solute flushing. Further development of regional-scale in situ sensor networks will provide better understanding of stormflow and solute generation across a wide range of landscape conditions.